{"title":"How reliable is the Real Adsorbed Solution Theory (RAST) for estimating ternary mixture equilibrium in microporous host materials?","authors":"Rajamani Krishna, Jasper M. van Baten","doi":"10.1016/j.fluid.2024.114260","DOIUrl":null,"url":null,"abstract":"<div><div>Microporous crystalline adsorbents such as zeolites, and metal-organic frameworks (MOFs) have potential use in a wide variety of separations applications. In applications such as CO<sub>2</sub> capture, the Ideal Adsorbed Solution Theory (IAST) often fails to provide a quantitative description of mixture adsorption equilibrium especially in cation-exchanged zeolites. The failure of the IAST is ascribable to non-compliance with one or more tenets mandated by the IAST such as (a) homogeneous distribution of adsorbates within the pore landscape, (b) no preferential location of guest species, and (c) absence of molecular clustering due to say hydrogen bonding. The focus of this article is on the reliability of the Real Adsorbed Solution Theory (RAST) models for quantitative estimation of adsorption equilibrium. Configurational-Bias Monte Carlo (CBMC) simulations are undertaken to determine the adsorption equilibrium for ternary CO<sub>2</sub>/CH<sub>4</sub>/N<sub>2</sub>, CO<sub>2</sub>/CH<sub>4</sub>/C<sub>3</sub>H<sub>8</sub>, CO<sub>2</sub>/CH<sub>4</sub>/H<sub>2</sub>, and water/methanol/ethanol mixtures in NaX, LTA-4A, CHA, DDR, and MFI zeolites. Additionally, CBMC simulations of the constituent binary pairs are used to determine the Wilson or NRTL parameters, taking due account of the dependence of the activity coefficients on the spreading pressure. Use of the binary pair Wilson or NRTL parameters allows the estimation of ternary mixture adsorption equilibrium, that is tested against the CBMC data on component loadings. In all investigated guest/host combinations, the RAST provides a good estimation of ternary mixture adsorption equilibrium.</div></div>","PeriodicalId":12170,"journal":{"name":"Fluid Phase Equilibria","volume":"589 ","pages":"Article 114260"},"PeriodicalIF":2.8000,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fluid Phase Equilibria","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0378381224002358","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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Abstract
Microporous crystalline adsorbents such as zeolites, and metal-organic frameworks (MOFs) have potential use in a wide variety of separations applications. In applications such as CO2 capture, the Ideal Adsorbed Solution Theory (IAST) often fails to provide a quantitative description of mixture adsorption equilibrium especially in cation-exchanged zeolites. The failure of the IAST is ascribable to non-compliance with one or more tenets mandated by the IAST such as (a) homogeneous distribution of adsorbates within the pore landscape, (b) no preferential location of guest species, and (c) absence of molecular clustering due to say hydrogen bonding. The focus of this article is on the reliability of the Real Adsorbed Solution Theory (RAST) models for quantitative estimation of adsorption equilibrium. Configurational-Bias Monte Carlo (CBMC) simulations are undertaken to determine the adsorption equilibrium for ternary CO2/CH4/N2, CO2/CH4/C3H8, CO2/CH4/H2, and water/methanol/ethanol mixtures in NaX, LTA-4A, CHA, DDR, and MFI zeolites. Additionally, CBMC simulations of the constituent binary pairs are used to determine the Wilson or NRTL parameters, taking due account of the dependence of the activity coefficients on the spreading pressure. Use of the binary pair Wilson or NRTL parameters allows the estimation of ternary mixture adsorption equilibrium, that is tested against the CBMC data on component loadings. In all investigated guest/host combinations, the RAST provides a good estimation of ternary mixture adsorption equilibrium.
期刊介绍：
Fluid Phase Equilibria publishes high-quality papers dealing with experimental, theoretical, and applied research related to equilibrium and transport properties of fluids, solids, and interfaces. Subjects of interest include physical/phase and chemical equilibria; equilibrium and nonequilibrium thermophysical properties; fundamental thermodynamic relations; and stability. The systems central to the journal include pure substances and mixtures of organic and inorganic materials, including polymers, biochemicals, and surfactants with sufficient characterization of composition and purity for the results to be reproduced. Alloys are of interest only when thermodynamic studies are included, purely material studies will not be considered. In all cases, authors are expected to provide physical or chemical interpretations of the results.
Experimental research can include measurements under all conditions of temperature, pressure, and composition, including critical and supercritical. Measurements are to be associated with systems and conditions of fundamental or applied interest, and may not be only a collection of routine data, such as physical property or solubility measurements at limited pressures and temperatures close to ambient, or surfactant studies focussed strictly on micellisation or micelle structure. Papers reporting common data must be accompanied by new physical insights and/or contemporary or new theory or techniques.
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